Extremely high-rate aqueous supercapacitor fabricated using doped carbon nanoflakes with large surface area and mesopores at near-commercial mass loading

作者:Mao, Nan; Wang, Huanlei*; Sui, Yang; Cui, Yongpeng; Pokrzywinski, Jesse; Shi, Jing; Liu, Wei; Chen, Shougang; Wang, Xin; Mitlin, David*
来源:Nano Research, 2017, 10(5): 1767-1783.
DOI:10.1007/s12274-017-1486-6

摘要

Achieving a satisfactory energy-power combination in a supercapacitor that is based on all-carbon electrodes and operates in benign aqueous media instead of conventional organic electrolytes is a major challenge. For this purpose, we fabricated carbon nanoflakes (20-100 nm in thickness, 5-mu m in width) containing an unparalleled combination of a large surface area (3,000 m(2).g(-1) range) and mesoporosity (up to 72%). These huge-surface area functionalized carbons (HSAFCs) also had a substantial oxygen and nitrogen content (similar to 10 wt.% combined), with a significant fraction of redox-active carboxyl/phenol groups in an optimized specimen. Their unique structure and chemistry resulted from a tailored single-step carbonization-activation approach employing (2-benzimidazolyl) acetonitrile combined with potassium hydroxide (KOH). The HSAFCs exhibited specific capacitances of 474 F.g(-1) at 0.5 A.g(-1) and 285 F.g(-1) at 100 A.g(-1) (charging time < 3 s) in an aqueous 2 M KOH solution. These values are among the highest reported, especially at high currents. When tested with a stable 1.8-V window in a 1 M Na2SO4 electrolyte, a symmetric supercapacitor device using the fabricated nanoflakes as electrodes yielded a normalized active mass of 24.4 Wh.kg(-1) at 223 W.kg(-1) and 7.3 Wh.kg(-1) at 9,360 W.kg(-1). The latter value corresponds to a charge time of <3 s. The cyclability of the devices was excellent, with 93% capacitance retention after 10,000 cycles. All the electrochemical results were achieved by employing electrodes with near-commercial mass loadings of 8 mg.cm(-2).